Catalytic Polysulfide Conversion and Physiochemical Confinement for Lithium–Sulfur Batteries

Catalytic Polysulfide Conversion and Physiochemical Confinement for Lithium–Sulfur Batteries

Advanced Energy Materials

10.1002/aenm.201904010

https://doi.org/10.1002/aenm.201904010

Zixu Sun, Sudarshan Vijay, Hendrik H. Heenen, Alex Yong Sheng Eng, Wenguang Tu, Yunxing Zhao, See Wee Koh, Pingqi Gao, Zhi Wei Seh, Karen Chan, Hong Li

Batteries

27 April 2020

Sun, Z., Vijay, S., Heenen, H. H., Eng, A. Y. S., Tu, W., Zhao, Y., Koh, S. W., Gao, P., Seh, Z. W., Chan, K., Li, H., Catalytic Polysulfide Conversion and Physiochemical Confinement for Lithium–Sulfur Batteries. Adv. Energy Mater. 2020, 10, 1904010. https://doi.org/10.1002/aenm.201904010

The lithium–sulfur (Li–S) battery is widely regarded as a promising energy storage device due to its low price and the high earth‐abundance of the materials employed. However, the shuttle effect of lithium polysulfides (LiPSs) and sluggish redox conversion result in inefficient sulfur utilization, low power density, and rapid electrode deterioration. Herein, these challenges are addressed with two strategies 1) increasing LiPS conversion kinetics through catalysis, and 2) alleviating the shuttle effect by enhanced trapping and adsorption of LiPSs. These improvements are achieved by constructing double‐shelled hollow nanocages decorated with a cobalt nitride catalyst. The N‐doped hollow inner carbon shell not only serves as a physiochemical absorber for LiPSs, but also improves the electrical conductivity of the electrode; significantly suppressing shuttle effect. Cobalt nitride (Co4N) nanoparticles, embedded in nitrogen‐doped carbon in the outer shell, catalyze the conversion of LiPSs, leading to decreased polarization and fast kinetics during cycling. Theoretical study of the Li intercalation energetics confirms the improved catalytic activity of the Co4N compared to metallic Co catalyst. Altogether, the electrode shows large reversible capacity (1242 mAh g−1 at 0.1 C), robust stability (capacity retention of 658 mAh g−1 at 5 C after 400 cycles), and superior cycling stability at high sulfur loading (4.5 mg cm−2).

PublisherCopyrights

This work was supported by Nanyang Technological University under NAP award (M408050000) and Singapore Ministry of Education Tier 1 program (2018-T1-001-051). S.V., H.H.H., and K.C. acknowledge a research grant (9455) from VILLUM FONDEN. Z.W.S acknowledges support from the Singapore National Research Foundation (NRF-NRFF2017-04).

This is the peer reviewed version of the following article: Sun, Z., Vijay, S., Heenen, H. H., Eng, A. Y. S., Tu, W., Zhao, Y., Koh, S. W., Gao, P., Seh, Z. W., Chan, K., Li, H., Catalytic Polysulfide Conversion and Physiochemical Confinement for Lithium–Sulfur Batteries. Adv. Energy Mater. 2020, 10, 1904010. https://doi.org/10.1002/aenm.201904010, which has been published in final form at https://doi.org/10.1002/aenm.201904010. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.

https://oar.a-star.edu.sg/communities-collections/articles/17440

1614-6840

Institute of Materials Research and Engineering